Controlling the synthesis of uniform electron-deficient Pd clusters for superior hydrogen production from formic acid

Ye, Wanyue; Pei, Wei; Zhao, Jijun; Huang, He; Li, Qian; Zhao, Jijun; Lu, Rongwen; Ge, Yuzhen; Zhang, Shufen

doi:10.1039/c9ta02035g

Cited by 44 publications

(38 citation statements)

References 45 publications

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“…3 [55] HCOONa in H 2 O at 80 °C 308 000 25 700 98 000 0.96 0.34 4 [56] NA in H 2 O at 60 °C 5 000 000 1900 98 000 0.06 12.18 5 [57] NA in H 2 O at 80 °C 2 400 000 171 000 125 000 0.16 0.25 6 [58] HCOONa 11 [64] NEt 3 in dioxane at 40 °C 100 000 653 168 000 5.09 108.99 12 [65] LiBF 4 in dioxane at 80 °C 983 642 196 728 g) 11 000 0.03 0.03 13 [66] HCOONa in neat HCOOH at 90 °C 2 160 000 13 320 e) 90 000 0.12 2.07 14 [67] NA in neat HCOOH at 95 °C 1 701 150 3067 158 000 0.28 15.51 15 [68] NA in H 2 O at 50 °C NA h) 18 625 f) 28 000 1.69 1.45…”

Section: Homogeneous Catalysismentioning

confidence: 99%

“…[77b] Interestingly, Ye et al have employed amine-modified SiO 2 , and graphene oxide (Pd@NH 2 -SiO 2 @NH 2 -GO, 15) for additive-free FA dehydrogenation to achieve a TOF of 18625 h −1 at 50 °C. [68] Such improved performance was attributed to NH 2 functionalities, which result in the formation of electron-deficient Pd clusters and also serve as proton reservoirs for dehydrogenation of FA.…”

Section: Heterogeneous Catalysismentioning

confidence: 99%

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Formic Acid to Power towards Low‐Carbon Economy

Dutta

Chatterjee

Cheng

et al. 2022

Advanced Energy Materials

136

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The corresponding global annual carbon dioxide (CO 2 ) emissions had also increased from 23.1 gigatonnes of CO 2 (Gt CO2 ) in 2000 to 33.2 Gt CO2 in 2018. The excessive reliance on fossil fuels has caused the atmospheric CO 2 concentration to increase from the pre-industrial 280 ppm in the 18th century to the annual average of more than 410 ppm nowadays, which is found to be positively correlated to climate change. [2] To alleviate the environmental issues and to find viable alternatives for depleting fossil fuel reserves, the development and largescale deployment of clean and sustainable energy systems is of utmost importance. The development of suitable energy carriers is necessary to enable energy storage and distribution and to overcome the deficiency due to the intermittency of renewable energy sources such as solar and wind power. The use of H 2 has a great potential to diversify energy sectors and to prepare for the future implementation of low-carbon electricity and renewable energy. H 2 fuel cell (FC) technology is considered mature and regarded as the only technology to realize mobility without change of habits. As stated in the 2019 report by International Energy Agency to G20, H 2 is expected "to play a key role in a clean, secure and affordable energy future." [3] However, due to the lack of viable technologies for safe, efficient, and economical storage and transportation of H 2 , the applications of hydrogen have significantly been limited. [4] The storage and utilization of low-carbon electricity and decarbonization of transportation are essential components for the future energy transition into a low-carbon economy. While hydrogen has been identified as a potential energy carrier, the lack of viable technologies for safe and efficient storage and transportation of H 2 greatly limits its applications and deployment at scale. Formic acid (FA) is considered one of the promising H 2 energy carriers because of its high volumetric H 2 storage capacity of 53 g H 2 /L, and relatively low toxicity and flammability for convenient and low-cost storage and transportation. FA can be employed to generate electricity either in direct FA fuel cells (FCs) or indirectly as an H 2 source for hydrogen FCs. FA can enable large-scale chemical H 2 storage to eliminate energy-intensive and expensive processes for H 2 liquefaction and compression and thus to achieve higher efficiency and broader utilization. This perspective summarizes recent advances in catalyst development for selective dehydrogenation of FA and high-pressure H 2 production. The advantages and limitations of FA-to-power options are highlighted. Existing life cycle assessment (LCA) and economic analysis studies are reviewed to discuss the feasibility and future potential of FA as a fuel.

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Section: Homogeneous Catalysismentioning

confidence: 99%

Section: Heterogeneous Catalysismentioning

confidence: 99%

Formic Acid to Power towards Low‐Carbon Economy

Dutta

Chatterjee

Cheng

et al. 2022

Advanced Energy Materials

136

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“…The production of hydrogen from FA proceeds via a dehydrogenation reaction (HCOOH ↔ H 2 + CO 2 ) that can be promoted by both homogeneous [ 12 , 13 ] and heterogeneous [ 14 , 15 , 16 ] catalysts, the latter being the preferred choice because of advantages associated with their use. The heterogeneous catalysts used in this reaction are frequently based on Pd nanoparticles supported on materials of diverse composition [ 6 , 17 , 18 , 19 , 20 , 21 , 22 ], with carbon materials being some of the most common supports [ 7 , 23 , 24 ]. Despite the vast literature reporting on Pd-carbon-based catalysts for the dehydrogenation of FA, most of the studies are aimed at optimizing the properties of the catalytic active phase (i.e., particle size [ 23 , 25 , 26 ], composition [ 17 , 27 , 28 , 29 , 30 ], etc.…”

Section: Introductionmentioning

confidence: 99%

H2 Production from Formic Acid Using Highly Stable Carbon-Supported Pd-Based Catalysts Derived from Soft-Biomass Residues: Effect of Heat Treatment and Functionalization of the Carbon Support

et al. 2021

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The production of hydrogen from liquid organic hydrogen carrier molecules stands up as a promising option over the conventional hydrogen storage methods. In this study, we explore the potential of formic acid as a convenient hydrogen carrier. For that, soft-biomass-derived carbon-supported Pd catalysts were synthesized by a H3PO4-assisted hydrothermal carbonization method. To assess the impact of the properties of the support in the catalytic performance towards the dehydrogenation of formic acid, three different strategies were employed: (i) incorporation of nitrogen functional groups; (ii) modification of the surface chemistry by performing a thermal treatment at high temperatures (i.e., 900 °C); and (iii) combination on both thermal treatment and nitrogen functionalization. It was observed that the modification of the carbon support with these strategies resulted in catalysts with enhanced performance and outstanding stability even after six consecutive reaction cycles, thus highlighting the important effect of tailoring the properties of the support.

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“…Despite the homogeneous catalysts based on Ir, Ru, and Fe organometallic complex usually have great catalytic activity and selectivity, while gold 25 , Platinum 26 , and palladium 4 well known heterogeneous catalysts used in the decomposition of FA. However, some reports have shown that nanostructure with base Pd such as Au 0.5 Pd 0.5 /NH 2 -N-rGO 27 , Pd-MIL-125 28 , Pd 1 Au 1 /30-LA 29 , AP-SiO 2 @PDA-NGO@Pd 30 , PdAu-MnOx/N-SiO 2 31 , CrAuPd/N-SiO 2 32 , IrPdAu/NH 2 -SBA-15 33 , Ag 0.2 Au 0.4 Pd 0.4 /rGO 34 , Au@Pd/UiO-66(Zr x Ti y ) 35 , Au–Pd/MIL-101 36 , and PdCoNi/TiO 2 37 , can efficiently decomposed FA under neat condition. Recently, our research group explored the catalytic application of Pd@Cu-MOF 38 and Pd@Cr-MOF 39 with open metal sites as an ideal Pd-catalyst for H 2 generation from FA in neat condition.…”

Section: Introductionmentioning

confidence: 99%

Anchoring Pd-nanoparticles on dithiocarbamate- functionalized SBA-15 for hydrogen generation from formic acid

Farajzadeh

Alamgholiloo

Nasibipour

et al. 2020

Sci Rep

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Hydrogen (H2) generation from natural biological metabolic products has remained a huge challenge for the energy arena. However, designing a catalytic system with complementary properties including high surface area, high loading, and easy separation offers a promising route for efficient utilization of nanoreactors for prospective H2 suppliers to a fuel cell. Herein, selective dehydrogenation of formic acid (FA) as a natural biological metabolic product to H2 and CO2 gas mixtures has been studied by supporting ultrafine palladium nanoparticles on organosulfur-functionalized SBA-15 nanoreactor under ultrasonic irradiation. The effects of the porous structure as a nanoreactor, and organosulfur groups, which presented around the Pd due to their prominent roles in anchoring and stabilizing of Pd NPs, studied as a superior catalyst for selective dehydrogenation of FA. Whole catalytic systems were utilized in ultrasonic irradiation in the absence of additives to provide excellent TOF/TON values. It was found that propose catalyst is a greener, recyclable, and more suitable option for the large-scale application and provide some new insights into stabilization of ultra-fine metal nanoparticle for a variety of applications.

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Controlling the synthesis of uniform electron-deficient Pd clusters for superior hydrogen production from formic acid

Abstract: The superior additives-free dehydrogenation of formic acid for hydrogen production by uniform electron-deficient Pd clusters.

Cited by 44 publications

References 45 publications

Formic Acid to Power towards Low‐Carbon Economy

Formic Acid to Power towards Low‐Carbon Economy

H2 Production from Formic Acid Using Highly Stable Carbon-Supported Pd-Based Catalysts Derived from Soft-Biomass Residues: Effect of Heat Treatment and Functionalization of the Carbon Support

Anchoring Pd-nanoparticles on dithiocarbamate- functionalized SBA-15 for hydrogen generation from formic acid

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